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1304
Introduction
Composite resins are commonly used dental restorative
materials, and significant improvements have been made in
their microstructure and properties (Cross et al., 1983; Jorden
and Suzuki, 1991; Bowen et al., 1992; Ferracane and Marker,
1992; Willems et al., 1992; Eick et al., 1993, 1997; Bayne et al.,
1994; Wilder et al., 1996; Loza-Herrero et al., 1998). To reinforce dental composite resins, short glass fibers have been
used as fillers, producing limited improvements in composite mechanical properties (Krause et al., 1989). Various other
filler systems have been tested for the reinforcement of composite resins (Antonucci et al., 1991). Particulates of networked fibers (Bayne and Thompson, 1996) were recently
used to strengthen composite resins. The effects of filler
level and degree of conversion on composite properties
have been examined (Condon and Ferracane, 1997). It is
generally suggested that direct-filling composite resins are
still susceptible to fracture and therefore are not recommended for use in large stress-bearing posterior applications, especially those that involve cusps (Ferracane, 1992;
Mazer et al., 1992; Sakaguchi et al., 1992; Bayne et al., 1994;
Leinfelder, 1995; Anusavice, 1996).
Reinforcement with ceramic single-crystalline whiskers
has been shown to toughen and strengthen engineering
structural materials (e.g., Lawn, 1993; Xu et al., 1996). These
whiskers are single crystals with a high degree of structural
perfection resulting in high strength values. The elongated
shapes of these whiskers (e.g., a length-to-diameter ratio of 5
to 10) can effectively bridge a matrix microcrack, restraining
it from propagating (Lawn, 1993; Xu et al., 1994). The small
whisker size (e.g., a diameter of 0.1 ,um to 1 ,um, two orders
of magnitude smaller than most ceramic fibers) facilitates a
relatively uniform distribution of the whiskers with random
orientation in the matrix, improves composite machinability
or polishability, and reduces abrasiveness (Xu et al., 1996).
Ceramic whiskers have been incorporated into matrices of
ceramics, metals, and some polymers, showing promising
reinforcement results (Tominaga and Sasaki, 1987; Carberry
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1305
Specimen fabrication
The silanized powder was manually blended by spatulation
with a resin monomer consisting of mass fractions of 48.975%
Bis-GMA, 48.975% TEGDMA (triethylene glycol dimethacrylate), 0.05% 2,6-di-tert-butyl-4-methylphenol (BHT), and 2%
benzoyl peroxide (BPO) to form paste one, the initiator paste, of
a two-part chemically activated composite. Paste two, the accelerator paste, consisted of the same amount of filler powder
mixed with a resin made of mass fractions of 49.5% Bis-GMA,
49.5% TEGDMA, and 1% N,N-dihydroxyethyl-p-toluidine
(DHEPT) as the polymerization accelerator. The following filler
mass fractions were tested so that the effect of whisker content
on composite properties could be evaluated: 0%, 10%, 20%,
30%, 40%, 45%, 50%, 55%, 60%, 65%, and 70%.
At each filler mass fraction, equal masses of the two pastes
were manually blended by spatulation and placed into a mold
cavity of 2 mm x 2 mm x 20 mm to make flexural specimens.
Each specimen was incubated at 37C for 15 min for chemical
curing, and then demolded. To examine the effect of degree of
conversion on composite mechanical properties, we subjected
additional specimens at a filler mass fraction of 70% to heat cure
at 90C for 24 hrs (Ferracane and Marker, 1992). The cured
specimens were immersed in distilled water at 37C for 24 hrs
prior to being tested.
Three control composites were fabricated. A hybrid composite (TPHTM, Caulk/Dentsply, Inc., Milford, DE, USA) consisted
of silanized silicate filler particles about 0.8 p.m in diameter and
a filler mass fraction of 78% in a matrix resin of a urethanemodified Bis-GMA and TEGDMA. A silica microfill composite,
fabricated in the present study, consisted of silanized silica particles 0.04 pm in size (Aerosil OX50, DEGUSSA Corp.,
Ridgefield, NJ, USA) at a filler mass fraction of 50% in a matrix
of Bis-GMA and TEGDMA mixed at a mass ratio of 1:1, the
same as that for the whisker composites. Since the whisker
pastes at filler mass fractions of less than 60% were relatively
flowable, a flowable composite (Ultraseal XT., Ultradent
Products, Inc., South Jordan, UT, USA) was also tested as control that contained barium fluorosilicate glass fillers to a mass
fraction of 60%. The control specimens were cured by light
(Triad 2000., Dentsply International, Inc., York, PA, USA) for 1
min on each side of the specimen. All the cured specimens were
immersed in distilled water at 37C for 24 hrs prior to being
tested.
Mechanical testing
A standard three-point flexural test (ASTM F417-78, 1984) with
a fixture span of 10 mm was used to fracture the specimens at a
crosshead speed of 0.5 mm/min on a computer-controlled
Universal Testing Machine (Model 5500R, Instron Corp.,
Canton, MA, USA). The specimen fracture surfaces were sputter-coated with gold and examined in a scanning electron
microscope (SEM, JSM-5300, JEOL, Inc., Peabody, MA, USA). A
Vickers diamond pyramid was used in a standard microhardness tester (Zwick of America, Inc., East Windsor, CT, USA) to
indent specimens at a normal load of 10 N. The impression
diagonal length was measured by means of an optical microscope with Nomarski contrast (Nikon Diaphot, Mager Scientific,
Inc., Dexter, MI, USA) coupled with a video micrometer (Model
305, Colorado Video, Inc., Boulder, CO, USA) (Xu et al., 1998).
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1306
Xu
250.
i
200
=150
O)
-hybrid
o
Isilica
L50
:flowable
20
40
60
(Ferracane
Greener,
Rueggeberg
et al., 1990; Ferracane
and
Three1986;
were made and tested
at each
Marker,and1992).
pellets
of the following whisker filler mass fractions: 0%, 10%, 20%,
30%, 40%, 50%, 60%, and 70%.
12
C
10
N*.
r/
hybrid
hyrdfilled
silica
flowable
..
20
40
80
60
1.1
-t
v 0.9
0.7
v
hybd
0.5
,
2
0.
0u.3
En
0.1
20
40
60
Measurement of polishability
To examine the effects of whiskers on the composite polishability, we prepared class I cavities in eight human third molars.
Four cavities were filled with the whisker composite resin having a filler mass fraction of 55%, and the other four cavities were
with the hybrid composite (TPH). The restorations were
polished simulating clinical procedures by means of a 12-fluted
carbide bur followed by a 30-fluted bur and finished with a rubber polishing tip. In addition, six bar specimens of each of the
two composites, with dimensions of 2 mm x 2 mm x 10 mm,
were fabricated according to the procedures described earlier
and polished by the same procedure as that used for the
restorations. The average surface roughness (Ra) and the maximum surface roughness (Rd) were measured by means of a
computer-controlled profilometry system (Perthometer
Concept, Mahr Corp., Cincinnati, OH, USA) with a trace length
of approximately 1 mm on each polished bar specimen.
One-way ANOVA was performed so that significance (c =
0.05) of composite properties could be detected. Tukey's
Multiple
Comparison Procedures were used at a family confidence coefficient of 0.95 to rank and group the measured values.
80
Results
Each datum in the plots of flexural strength, modulus, and
hardness (Fig. 1) is the mean value with error bar showing
Oone standard deviation of six measurements. The silica
Figure 1. Each datum is the mean value with one standard deviation;
n = 6. A hybrid posterior composite (TPH) at a filler mass fraction of
78%, a microfill (silica) at a filler mass fraction of 50%, and a flowable
composite (Ultraseal) at a filler mass fraction of 60% are included as
control. The open square symbol in each plot designates the whisker
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composite at a filler mass fraction of 50%, the flowable composite (Ultraseal) at a filler mass
fraction of 60%, and the hybrid
posterior composite (TPH) at a
filler mass fraction of 78'$ are
included as control. The open
square symbol in each plot designates additional whisker composite specimens at a filler mass fraction of 70% that was
heat-cured. The modulus and hardness showed a monotonic increase with an increase in the filler level. The flexural
strength of the whisker composite increased from about 100
MPa to almost 200 MPa with an increase in the filler level
from Oh to 45%, then plateaued and even slightly
decreased when the filler level was further increased to
70/. The whisker composite with a filler mass fraction of
55'Y, had a flexural strength (mean + one standard deviation; n = 6) of 196 + 10 MPa, significantly higher than 83 +
14 MPa of the microfill composite (silica) and 120 16 MPa
of the hybrid composite (TPH) (family confidence coefficient = 0.95; Tukey's multiple-comparison test). Heat-cured
specimens had significantly higher flexural strength and
hardness than those without heat-curing at a filler mass
fraction of 70% (p < 0.05; Student's t).
Representative SEM micrographs of specimen fracture
surfaces (Fig. 2) are for (A) the hybrid composite (TPH), (B)
the unfilled resin (filler mass fraction 0%), (C) the whisker
composite with a filler mass fraction of 10%, and (D) the
whisker composite with a filler mass fraction of 45%. The
crack propagation direction during the flexural test was
approximately from top to bottom of each micrograph. The
fracture surfaces of the hybrid composite and the unfilled
resin were relatively flat; those of the whisker composites
had relatively large fracture steps, as indicated by the big
Figure 3. Higher-magnification SEM of fracture surfaces of the
whisker composite with a filler mass fraction of 55'Y. The direction
of crack propagation during flexural failure was approximately from
top to bottom of each micrograph. (A) Whisker pinninlg and deflecting the crack. When the crack finally broke away from the whisker,
numerous fracture lines and steps were created in the resin fracture
surface. (B) Whiskers pulled out of the matrix during crack opening.
The small arrows in Fig. 3B indicate remnants of matrix resin on the
surfaces of the whiskers, suggesting energy consumption and friction during whisker pullout.
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I130(7
1308
Xut
70 heat-cured
conversion at a filler mass fraction of 0% was significantly higlher than that at 707,o; the degree of conversion at a
filler mass fraction of 70% with heat-cure was significantly higher
than that without heat-cure (p < 0.05; Student's t).
T he degree of
procedures,
were not
cantly different (p
signifi-
>
0.1;
Student's t).
Discussion
D
03
-9
I
200
150
E=L
.n
0.75
(U
100
p
to
:3
0
0.50
C4
U-
1.00
50
0
0
1.
c-n
0
-.2
0.25
0.
k;
,a4
--a
Figure 4. Restorations of (A) a hybrid composite control (TPH), and (B) a whisker composite with a
filler mass fraction of 55%. The restorations appeared smooth and shiny after clinical polishing. The
whisker composite was relatively opaque with a whitish color. (C) Flexural strength of the two composites. (D) Average (R,) and maximum (R,) surface roughness values of bar specimens polished
simulating clinical procedures. Horizontal lines indicate values (mean + SD; n = 6) that are not significantly different (p > 0.1; Student's t).
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1309
Acknowledgments
The author is grateful to Drs. F.C. Eichmiller and J.M.
Antonucci for fruitful discussions, J.W. Stansbury for help
in the degree of conversion measurement, G.E. Schumacher
for tooth cavity restorations, and H. Liao for statistical
analysis. This study was supported by NIDCR grants P 50
DE09322 and R29 DE12476, NIST, and the ADAHF.
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1310
Xu
Disclaimer
Certain commercial materials and equipment are identified
in this paper to specify the experimental procedure. In no
instance does such identification imply recommendation or
endorsement by the National Institute of Standards and
Technology or the ADA Health Foundation or that the
material or equipment identified is necessarily the best
available for the purpose.
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